Just Accepted Articles have been posted online after technical editing and typesetting for immediate view. The final edited version with page numbers will appear in the Current Issue soon.
In summary, Liu etal. realized the thermally-induced spin transition with colossal PTE and NTE properties in a cyano-bridged hexanuclear complex. The spin transition as well as the conformational transformation triggered anisotropic alteration of the rhombic {FeIII2FeII2} unit and modifications in intermolecular C–H···π interactions, ultimately resulting in NTE along the b axis. This work demonstrates that merging SCO compounds with a pliable rhombic structure and intermolecular interactions leads to exceptional structural and thermodynamic characteristics. This approach represents a significant strategy in the realm of crystal engineering and thermo-responsive molecular devices.